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Hypothesis: A sustainable dynamic anti-icing surface with the potential for rapid rechargeability 假设:具有快速充电潜力的可持续动态防冰表面
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-04 DOI: 10.1016/j.jcis.2024.11.009
Xinshu Zou , Feng Wang , Jianying He , Zhiliang Zhang
Ice accumulation poses significant challenges across numerous industries. While dynamic anti-icing surfaces (DAIS) have shown potential in mitigating ice formation and adhesion, their practical use is often limited by the rapid diffusion of liquids and lack of reusability. Overcoming these limitations is crucial to addressing the environmental and economic issues related to ice management. In this study, we introduce a novel approach by incorporating β-cyclodextrin (β-CD) into polydimethylsiloxane (PDMS) silicone rubber, enabling the creation of a sustainable DAIS with the potential of rapid rechargeability. The multiple hydroxyl groups present on the outer surface of β-CD facilitate dipole–dipole interactions and hydrogen bonding, particularly with polar molecules like ethanol and isopropanol. This transforms the surface into a rechargeable system, capable of restoring its low ice adhesion functionality within just 10 min after liquid replenishment. When ice forms on the surface, the system dynamically responds to environmental changes via concentration gradients, controlling the release of liquids and altering surface characteristics. These retained liquids effectively lower the freezing point, melt the ice, and disrupt the ice structure, converting the solid–liquid interface into a liquid–liquid interface. The DAIS effectively alter the ice-substrate interaction and enhance performance at temperatures as low as −18 ℃. By optimizing the β-CD mass ratio and liquid treatments, especially with isopropanol, we achieved an ultra-low ice adhesion strength of 0.6 kPa, which remains stable even after 35 days. This study presents a significant advancement in the development of sustainable, rapidly rechargeable DAIS, offering immense potential for applications in various industries.
积冰给众多行业带来了巨大挑战。虽然动态防冰表面(DAIS)在减少冰的形成和附着方面已显示出潜力,但其实际使用往往受到液体快速扩散和缺乏可重复使用性的限制。克服这些限制对于解决与冰管理相关的环境和经济问题至关重要。在本研究中,我们引入了一种新方法,将 β-环糊精(β-CD)融入聚二甲基硅氧烷(PDMS)硅橡胶中,从而创造出一种具有快速充电潜力的可持续 DAIS。β-CD 外表面的多个羟基促进了偶极-偶极相互作用和氢键,特别是与乙醇和异丙醇等极性分子的相互作用和氢键。这使表面变成了一个可充电系统,能够在补充液体后 10 分钟内恢复其低冰粘附功能。当表面结冰时,系统会通过浓度梯度对环境变化做出动态响应,控制液体的释放并改变表面特性。这些滞留的液体能有效降低冰点,融化冰层,破坏冰层结构,将固液界面转化为液液界面。DAIS 有效地改变了冰与基底的相互作用,提高了在-18 ℃低温下的性能。通过优化 β-CD 质量比和液体处理,特别是异丙醇处理,我们获得了 0.6 kPa 的超低冰粘附强度,即使在 35 天后也能保持稳定。这项研究在开发可持续、快速充电的 DAIS 方面取得了重大进展,为各行各业的应用提供了巨大潜力。
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引用次数: 0
Heterointerfacial engineering of N,P-doped carbon nanosheets supported Co/Co2P nanoparticles for boosting oxygen reduction and oxygen evolution reactions towards rechargeable Zn-air battery 支持 Co/Co2P 纳米粒子的 N、P-掺杂碳纳米片的异界面工程,用于促进可充电锌-空气电池的氧还原和氧进化反应。
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-04 DOI: 10.1016/j.jcis.2024.11.011
Wenhao Xi , Tongchen Wu , Pan Wang , Wenlong Huang , Bifen Gao , Liwen He , Yilin Chen , Bizhou Lin
Transition metal phosphides (TMPs) with high electrocatalytic activity for the oxygen evolution reaction (OER) are reckoned as a substitution of precious group metals catalysts in rechargeable Zn-air battery. In this work, Co/Co2P heterojunction nanoparticles supported N,P-doped carbon nanosheets (Co/Co2P@NPCNS) were designed and prepared via a facile one-step molten salt-assisted pyrolysis process. Density function theory calculations reveal that the heterogeneous interactions of Co/Co2P effectively enhance the bifunctional electrocatalytic activity for oxygen reduction reaction (ORR) and OER. The synergistic interaction between the Co/Co2P heterojunction nanoparticles with highly exposed active sites and excellent catalytic activity and the two-dimensional doped carbon nanosheets with high conductivity contributes to Co/Co2P@NPCNS exhibiting preeminent bifunctional ORR/OER activity and stability with a high half-wave potential for ORR (0.87 V), a low overpotential for OER (302 mV at 10 mA cm−2) and a low potential gap (0.66 V). The homemade rechargeable Zn-air battery performs high peak power density (187 mW cm−2) and exceptional endurance. This heterogeneous interface tactic of integrating TMPs with heteroatom-doped carbon materials may shed light on the research and development of non-precious metal electrocatalysts.
在氧进化反应(OER)中具有高电催化活性的过渡金属磷化物(TMPs)被认为是可充电锌-空气电池中贵族金属催化剂的替代品。在这项工作中,通过一步熔盐辅助热解工艺,设计并制备了支持 N、P 掺杂碳纳米片的 Co/Co2P 异质结纳米粒子(Co/Co2P@NPCNS)。密度函数理论计算表明,Co/Co2P 的异质相互作用有效地提高了氧还原反应(ORR)和 OER 的双功能电催化活性。具有高暴露活性位点和优异催化活性的 Co/Co2P 异质结纳米粒子与具有高导电性的二维掺杂碳纳米片之间的协同作用,使得 Co/Co2P@NPCNS 具有卓越的 ORR/OER 双功能活性和稳定性,ORR 半波电位高(0.87 V),OER 过电位低(10 mA cm-2 时为 302 mV),电位差低(0.66 V)。自制的可充电锌空气电池具有峰值功率密度高(187 mW cm-2)和超强的续航能力。这种将 TMPs 与掺杂杂原子的碳材料结合在一起的异质界面战术可能会为非贵金属电催化剂的研究和开发带来启示。
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引用次数: 0
Heterojunction-structured Ni0.85Se/CoSe nanoparticles anchored on holey graphene for performance-enhanced sodium-ion batteries 锚定在孔状石墨烯上的异质结结构 Ni0.85Se/CoSe 纳米粒子用于性能增强型钠离子电池。
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-04 DOI: 10.1016/j.jcis.2024.11.012
Shenghua Hou , Fei Xie , Xuejie Wang , Liuyang Zhang , Xinming Nie , Jiaguo Yu , Tao Liu
Graphene-based metal selenides, are increasingly recognized for their potential in sodium-ion battery applications due to their superior electrochemical properties. The unique structure of graphene facilitates rapid in-plane transport of sodium ions, but the interlayer diffusion remains a significant challenge. The Ni0.85Se@CoSe heterojunctions, strategically grown adjacent to the graphene pores, offer a novel solution by creating in-plane holes that serve as direct channels for vertical ion transport, thereby enhancing cross-layer sodium ion permeation. The incorporation of Ni0.85Se@CoSe heterojunctions with holey graphene (NCS/HG) significantly enhances the reaction dynamics between sodium ions and anode material. These heterojunctions not only promote easier sodium ion insertion/extraction process by reducing the Na+ adsorption energy, but also improve the electrical conductivity by adjusting the band gap. The configuration supports high current density applications (573.5 mAh/g at 5.0 A/g), and ensures robust cycle stability with a capacity retention rate of 97 % after 1000 cycles at 2.0 A/g. Therefore, the development and etching techniques employed in engineering the Ni0.85Se@CoSe/HG graphene-based anodes exemplify a significant advancement in anode material design, highlighting the importance of material architecture in the development of high-performance energy storage devices.
石墨烯基金属硒化物因其卓越的电化学特性,在钠离子电池应用中的潜力日益得到认可。石墨烯的独特结构有利于钠离子在平面内的快速传输,但层间扩散仍是一个重大挑战。在石墨烯孔隙附近战略性生长的 Ni0.85Se@CoSe 异质结提供了一种新颖的解决方案,它能产生平面内孔,作为离子垂直传输的直接通道,从而增强钠离子的跨层渗透。Ni0.85Se@CoSe异质结与孔状石墨烯(NCS/HG)的结合大大增强了钠离子与阳极材料之间的反应动力学。这些异质结不仅通过降低 Na+ 吸附能来简化钠离子的插入/萃取过程,还通过调整带隙来提高导电性。这种配置支持高电流密度应用(5.0 A/g 时为 573.5 mAh/g),并确保了强大的循环稳定性,在 2.0 A/g 下循环 1000 次后容量保持率为 97%。因此,Ni0.85Se@CoSe/HG 石墨烯基阳极工程中采用的开发和蚀刻技术体现了阳极材料设计的重大进步,突出了材料结构在开发高性能储能设备中的重要性。
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引用次数: 0
Manipulating the d- and p-Band centers of amorphous alloys by variable composition for robust oxygen evolution reaction 通过改变成分操纵非晶合金的 d 波段和 p 波段中心,以实现稳健的氧进化反应。
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-04 DOI: 10.1016/j.jcis.2024.11.007
Yuci Xin , Yong Wu , Xingan Dong , Yuhan Li , Zhenxiang Cheng , Jianli Wang , Xiaolong Guo , Peng Yu
Amorphous electrocatalysts display several unique advantages in electricity-driven water splitting compared to their crystalline analogs, but understanding their structure–activity relationships remains a major challenge. Herein, we show that the d- and p-electronic states of amorphous Ni-Fe-B can be subtly manipulated by varying the Ni and Fe contents. The optimal Ni-Fe-B alloy exhibits a high performance in the oxygen evolution reaction (OER), as supported by its impressive stability (no clear degradation after 100 h) and considerably lower overpotential compared to those of its crystalline analogs. Based on theoretical calculations, different Ni and Fe contents can cause significant shifts in the d-band levels of Ni and Fe and the p-band level of B, thus altering the OER activity. Additionally, the energy difference between the d- and p-band centers (ΔEad-p) may be an effective index for use in reflecting the structure–activity relationship of an amorphous Ni-Fe-B alloy in the OER. An amorphous Ni-Fe-B alloy with a smaller ΔEad-p displays a higher intrinsic activity. This study supplies a unique direction for use in constructing the structure–activity relationships of amorphous electrocatalysts by revealing the role of ΔEad-p, which promotes fundamental research and the practical application of amorphous electrocatalysts.
与晶体催化剂相比,非晶态电催化剂在电力驱动的水分离方面具有一些独特的优势,但了解其结构与活性之间的关系仍然是一项重大挑战。在此,我们展示了通过改变镍和铁的含量可以巧妙地操纵非晶态镍-芴-B 的 d 电子态和 p 电子态。最佳的 Ni-Fe-B 合金在氧进化反应(OER)中表现出很高的性能,这得益于它令人印象深刻的稳定性(100 小时后无明显降解)以及与其晶体类似物相比低得多的过电位。根据理论计算,不同的镍和铁含量会导致镍和铁的 d 波段水平以及 B 的 p 波段水平发生显著变化,从而改变 OER 的活性。此外,d 波段和 p 波段中心的能量差(ΔEad-p)可能是反映非晶镍铁合金在 OER 中的结构-活性关系的有效指标。ΔEad-p越小的非晶态镍-铁-B合金显示出越高的内在活性。该研究通过揭示ΔEad-p的作用,为构建非晶态电催化剂的结构-活性关系提供了一个独特的方向,促进了非晶态电催化剂的基础研究和实际应用。
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引用次数: 0
Enhanced bifunctional electrocatalysis of Co5.47N nanocrystals in porous carbon nanofibers for high-efficiency zinc-air batteries 增强多孔碳纳米纤维中 Co5.47N 纳米晶体的双功能电催化,用于高效锌-空气电池。
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-03 DOI: 10.1016/j.jcis.2024.10.201
Bin Qiao, Jing Zhang, Xuhui Li, Xingming Ning, Zhongwei An, Xinbing Chen, Yu Chen, Pei Chen
As a promising energy conversion and storage device, recently, rechargeable zinc-air batteries (ZABs) have developed rapidly, and the exploitation of excellent electrode catalysts to improve the energy efficiency and long-term performance of ZABs has become a focus of current research. Herein, the Co5.47N nanocrystals embedded in porous carbon nanofibers (Co5.47N PCNFs) were designed to act as a bifunctional electrocatalyst for the oxygen reduction reaction (ORR) and iodide oxidation reaction (IOR), which occur on the electrode in the charging-discharging process of ZABs. The electrochemistry results showed that the ORR activity of Co5.47N PCNFs is comparable to the commercial Pt/C electrocatalyst, and the IOR activity and stability are higher than those of the Pt/C electrocatalyst. Importantly, Co5.47N PCNFs electrocatalyst endows ZABs with a low charge–discharge voltage difference (0.49 V), a high round-trip energy efficiency (72.1 %), as well as a large specific capacity (791.5 mAh gZn−1), surpassing the performance of Pt/C electrocatalyst. Density functional theory calculation demonstrates that Co5.47N PCNFs have lower Gibbs free energy for the formation of IOR intermediate species, thereby displaying outstanding IOR catalytic performance compared to that of Pt/C electrocatalyst. These findings offer crucial insights into the rational design of cobalt nitride-based electrocatalysts for application in ZABs with high energy efficiency.
作为一种前景广阔的能量转换和储存装置,可充电锌空气电池(ZABs)近来发展迅速,如何利用优异的电极催化剂来提高 ZABs 的能量效率和长期性能已成为当前研究的重点。本文设计了嵌入多孔碳纳米纤维中的 Co5.47N 纳米晶体(Co5.47N PCNFs)作为双功能电催化剂,用于 ZABs 充放电过程中电极上发生的氧还原反应(ORR)和碘氧化反应(IOR)。电化学结果表明,Co5.47N PCNFs 的 ORR 活性与商用 Pt/C 电催化剂相当,IOR 活性和稳定性均高于 Pt/C 电催化剂。重要的是,Co5.47N PCNFs 电催化剂赋予了 ZABs 较低的充放电电压差(0.49 V)、较高的往返能量效率(72.1 %)和较大的比容量(791.5 mAh gZn-1),其性能超过了 Pt/C 电催化剂。密度泛函理论计算表明,Co5.47N PCNFs 在形成 IOR 中间物种时具有较低的吉布斯自由能,因此与 Pt/C 电催化剂相比,具有出色的 IOR 催化性能。这些发现为合理设计基于氮化钴的电催化剂提供了重要启示,使其在 ZAB 中的应用具有高能效。
{"title":"Enhanced bifunctional electrocatalysis of Co5.47N nanocrystals in porous carbon nanofibers for high-efficiency zinc-air batteries","authors":"Bin Qiao,&nbsp;Jing Zhang,&nbsp;Xuhui Li,&nbsp;Xingming Ning,&nbsp;Zhongwei An,&nbsp;Xinbing Chen,&nbsp;Yu Chen,&nbsp;Pei Chen","doi":"10.1016/j.jcis.2024.10.201","DOIUrl":"10.1016/j.jcis.2024.10.201","url":null,"abstract":"<div><div>As a promising energy conversion and storage device, recently, rechargeable zinc-air batteries (ZABs) have developed rapidly, and the exploitation of excellent electrode catalysts to improve the energy efficiency and long-term performance of ZABs has become a focus of current research. Herein, the Co<sub>5.47</sub>N nanocrystals embedded in porous carbon nanofibers (Co<sub>5.47</sub>N PCNFs) were designed to act as a bifunctional electrocatalyst for the oxygen reduction reaction (ORR) and iodide oxidation reaction (IOR), which occur on the electrode in the charging-discharging process of ZABs. The electrochemistry results showed that the ORR activity of Co<sub>5.47</sub>N PCNFs is comparable to the commercial Pt/C electrocatalyst, and the IOR activity and stability are higher than those of the Pt/C electrocatalyst. Importantly, Co<sub>5.47</sub>N PCNFs electrocatalyst endows ZABs with a low charge–discharge voltage difference (0.49 V), a high round-trip energy efficiency (72.1 %), as well as a large specific capacity (791.5 mAh g<sub>Zn</sub><sup>−1</sup>), surpassing the performance of Pt/C electrocatalyst. Density functional theory calculation demonstrates that Co<sub>5.47</sub>N PCNFs have lower Gibbs free energy for the formation of IOR intermediate species, thereby displaying outstanding IOR catalytic performance compared to that of Pt/C electrocatalyst. These findings offer crucial insights into the rational design of cobalt nitride-based electrocatalysts for application in ZABs with high energy efficiency.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 ","pages":"Pages 469-478"},"PeriodicalIF":9.4,"publicationDate":"2024-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142611338","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Specific smart sensing of electron-rich antibiotics or histidine improves the antenna effect, luminescence, and photodynamic sterilization capabilities of lanthanide polyoxometalates 富电子抗生素或组氨酸的特异性智能感应提高了镧系聚氧金属酸盐的天线效应、发光和光动力杀菌能力。
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-03 DOI: 10.1016/j.jcis.2024.11.006
Meng-Juan Tang , Zhong-Hong Zhu , Yun-Lan Li , Wen-Wen Qin , Fu-Pei Liang , Hai-Ling Wang , Hua-Hong Zou
Excessive discharge of antibiotics seriously threatens human health and is thus a global public health problem. This highlights the urgent need to develop intelligent sensing materials for specific antibiotics that are highly visual, fast, convenient, and inexpensive. Herein, two reverse α-octamolybdate polyoxometalates (POMs; Mo8) were used to chelate lanthanide ions to obtain lanthanide POMs (LnPOMs; LnMo16; Ln = Eu, Sm, Tb, Gd) with highly sensitive smart photoresponses to specific antibiotics (ofloxacin [OFN], norfloxacin [NOR], enrofloxacin [ENR], and oxytetracycline [OTC]) and histidine (His) with luminescence turn-on. Specific antibiotics and His, which has an electron-rich structure, can efficiently enhance the antenna effect, thereby greatly improving the luminescence of EuMo16. Surprisingly, OFN and NOR both enhanced the luminescence of Eu(III) ions and Mo8, whereas ENR and OTC only enhanced the luminescence of Eu(III) ions, showing a differentiated sensitization effect. More notably, the combination of POMs and Ln(III) ions enhanced the ability of LnPOMs to produce reactive oxygen species under light irradiation, and these LnPOMs showed significant sterilization effects on Escherichia coli and Staphylococcus aureus. To our knowledge, this is the first time electron-rich antibiotics or amino acids were used to enhance the luminescence of LnPOMs, achieving luminescence-enhanced photoresponse to specific antibiotics and amino acids.
抗生素的过量排放严重威胁人类健康,因而是一个全球性的公共卫生问题。因此,开发可视性强、快速、方便、廉价的特定抗生素智能传感材料迫在眉睫。在此,我们利用两种反向α-辛钼酸盐聚氧金属盐(POMs;Mo8)与镧离子螯合,得到了镧系元素 POMs(LnPOMs;LnMo16;Ln=Eu、Sm、Tb、Gd),它们对特定抗生素(氧氟沙星[OFN]、诺氟沙星[NOR]、恩诺沙星[ENR]和土霉素[OTC])和组氨酸(His)具有高灵敏度的智能光响应,并开启发光。特定的抗生素和具有富电子结构的 His 可以有效地增强天线效应,从而大大提高 EuMo16 的发光性能。令人惊讶的是,OFN 和 NOR 都能增强 Eu(III)离子和 Mo8 的发光,而 ENR 和 OTC 则只能增强 Eu(III)离子的发光,显示出不同的敏化效果。更值得注意的是,POMs 与 Ln(III) 离子的结合增强了 LnPOMs 在光照射下产生活性氧的能力,这些 LnPOMs 对大肠杆菌和金黄色葡萄球菌有显著的杀菌效果。据我们所知,这是首次利用富电子抗生素或氨基酸来增强 LnPOMs 的发光,实现了对特定抗生素和氨基酸的发光增强光反应。
{"title":"Specific smart sensing of electron-rich antibiotics or histidine improves the antenna effect, luminescence, and photodynamic sterilization capabilities of lanthanide polyoxometalates","authors":"Meng-Juan Tang ,&nbsp;Zhong-Hong Zhu ,&nbsp;Yun-Lan Li ,&nbsp;Wen-Wen Qin ,&nbsp;Fu-Pei Liang ,&nbsp;Hai-Ling Wang ,&nbsp;Hua-Hong Zou","doi":"10.1016/j.jcis.2024.11.006","DOIUrl":"10.1016/j.jcis.2024.11.006","url":null,"abstract":"<div><div>Excessive discharge of antibiotics seriously threatens human health and is thus a global public health problem. This highlights the urgent need to develop intelligent sensing materials for specific antibiotics that are highly visual, fast, convenient, and inexpensive. Herein, two reverse α-octamolybdate polyoxometalates (POMs; <strong>Mo<sub>8</sub></strong>) were used to chelate lanthanide ions to obtain lanthanide POMs (LnPOMs; <strong>LnMo<sub>16</sub></strong>; Ln = Eu, Sm, Tb, Gd) with highly sensitive smart photoresponses to specific antibiotics (ofloxacin [OFN], norfloxacin [NOR], enrofloxacin [ENR], and oxytetracycline [OTC]) and histidine (His) with luminescence turn-on. Specific antibiotics and His, which has an electron-rich structure, can efficiently enhance the antenna effect, thereby greatly improving the luminescence of <strong>EuMo<sub>16</sub></strong>. Surprisingly, OFN and NOR both enhanced the luminescence of Eu(III) ions and <strong>Mo<sub>8</sub></strong>, whereas ENR and OTC only enhanced the luminescence of Eu(III) ions, showing a differentiated sensitization effect. More notably, the combination of POMs and Ln(III) ions enhanced the ability of LnPOMs to produce reactive oxygen species under light irradiation, and these LnPOMs showed significant sterilization effects on <em>Escherichia coli</em> and <em>Staphylococcus aureus</em>. To our knowledge, this is the first time electron-rich antibiotics or amino acids were used to enhance the luminescence of LnPOMs, achieving luminescence-enhanced photoresponse to specific antibiotics and amino acids.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 ","pages":"Pages 235-246"},"PeriodicalIF":9.4,"publicationDate":"2024-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142589587","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Modular hydrogel selectively adsorbs phosphates and hexavalent chromium while enabling phosphate recovery 模块化水凝胶可选择性地吸附磷酸盐和六价铬,同时实现磷酸盐回收。
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-03 DOI: 10.1016/j.jcis.2024.11.005
Miao Su, Jiabao Hu, ZiSheng Liu, Sicheng Liu, Binsong Wang
Electroplating wastewater containing high concentrations of phosphates and hexavalent chromium Cr(VI) poses serious environmental pollution. Moreover, phosphorus, as a non-renewable resource, necessitates its recovery to meet sustainable development goals. To address this issue, this study used sodium alginate as the scaffold module, synthesized lanthanum carbonate in situ within a chitosan module to serve as the phosphate adsorption module, and employed polyethyleneimine (PEI) modules to enhance the adsorption capacity for Cr(VI), successfully fabricating a modular hydrogel (LC-CSP). LC-CSP exhibits a complex porous structure and surface morphology, forming an ultra-low-density fiber network with good strength and elasticity, ensuring uniform distribution and exposure of active sites. Under optimal conditions for single-component adsorption, LC-CSP achieved adsorption capacities of 232.02 mg/g for phosphates and 474.61 mg/g for Cr(VI). Additionally, LC-CSP demonstrated excellent reusability, retaining over 83 % of its performance after five cycles. In simulated electroplating wastewater experiments with various interfering substances, LC-CSP maintained high removal efficiencies (>90.72 %) for phosphates and Cr(VI). Post-experiment, enriched water after phosphate desorption was further treated to recover phosphorus resources in complex water environments. Multiple characterization techniques elucidated the adsorption mechanisms of LC-CSP: phosphate adsorption primarily involved ligand exchange, electrostatic interactions, and hydrogen bonding, while Cr(VI) adsorption included electrostatic interactions, hydrogen bonding, and reduction reactions. Finally, fixed-bed simulated wastewater adsorption experiments validated the technical potential of LC-CSP for practical electroplating wastewater management.
含有高浓度磷酸盐和六价铬 Cr(VI) 的电镀废水造成了严重的环境污染。此外,磷作为一种不可再生资源,有必要对其进行回收,以实现可持续发展目标。针对这一问题,本研究采用海藻酸钠作为支架模块,在壳聚糖模块中原位合成碳酸镧作为磷酸盐吸附模块,并采用聚乙烯亚胺(PEI)模块增强对六价铬的吸附能力,成功制备了一种模块化水凝胶(LC-CSP)。LC-CSP 具有复杂的多孔结构和表面形态,形成了具有良好强度和弹性的超低密度纤维网,确保了活性位点的均匀分布和暴露。在单组分吸附的最佳条件下,LC-CSP 对磷酸盐的吸附容量为 232.02 mg/g,对六价铬的吸附容量为 474.61 mg/g。此外,LC-CSP 还具有极佳的重复利用率,经过五个循环后,其性能保持率超过 83%。在含有各种干扰物质的模拟电镀废水实验中,LC-CSP 对磷酸盐和六(七)铬保持了较高的去除率(>90.72%)。实验后,对磷酸盐解吸后的富集水进行了进一步处理,以回收复杂水环境中的磷资源。多种表征技术阐明了 LC-CSP 的吸附机理:磷酸盐的吸附主要涉及配体交换、静电作用和氢键,而六价铬的吸附则包括静电作用、氢键和还原反应。最后,固定床模拟废水吸附实验验证了 LC-CSP 在实际电镀废水处理中的技术潜力。
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引用次数: 0
Fullerenols as efficient ferroptosis inhibitor by targeting lipid peroxidation for preventing drug-induced acute kidney injury 富勒烯醇通过靶向脂质过氧化作用成为高效的铁氧化抑制剂,可预防药物引起的急性肾损伤
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-03 DOI: 10.1016/j.jcis.2024.10.198
Wei Chen , Bing Wang , Shanshan Liang , Lingna Zheng , Hao Fang , Si Xu , Tingfeng Zhang , Meng Wang , Xiao He , Weiyue Feng
Acute kidney injury (AKI) is characterized by rapid and significant deterioration of renal function over a short duration with high mortality. However, the intricate pathophysiological mechanisms underlying AKI have hindered the development of effective therapeutic strategies. Recent research has highlighted the crucial role of ferroptosis in the pathogenesis of AKI and has identified it as a promising therapeutic target. Herein, we investigated the prophylactic efficacy of fullerenol nanoparticles, renowned for their broad-spectrum free radical scavenging capabilities and favorable biocompatibility, in preventing and mitigating ferroptosis-mediated cisplatin-induced AKI. Our findings demonstrate the remarkable potential of fullerenols in mitigating AKI. Specifically, fullerenols exert their protective effects primarily by suppressing renal lipid peroxidation and ferrous iron accumulation, which are two defining hallmarks of ferroptosis. Notably, fullerenols significantly inhibited the upregulation of key enzymes involved in the intracellular lipid peroxidation induced by cisplatin, including acyl-coA synthetase long chain family member 4 (ACSL4), arachidonate lipoxygenase 3 (ALOXE3), and cytochrome P450 oxidoreductase (POR), and enhanced antioxidant systems xc-/Glutathione (GSH)/Glutathione Peroxidase 4 (GPX4). Fullerenols also significantly suppressed the increase in mRNA expression of iron regulation-related genes and prevented the elevation of low-valent iron levels in the kidney tissue of AKI mice. Collectively, our study presents fullerenol as a promising drug candidate for the prevention of AKI in clinical settings, and provides valuable insights into the management of various ferroptosis-associated diseases.
急性肾损伤(AKI)的特点是肾功能在短时间内迅速显著恶化,死亡率高。然而,AKI 的病理生理机制错综复杂,阻碍了有效治疗策略的开发。最近的研究强调了铁蛋白沉积在 AKI 发病机制中的关键作用,并将其确定为一个有前景的治疗靶点。在此,我们研究了富勒烯醇纳米颗粒在预防和减轻铁蛋白沉积介导的顺铂诱导的 AKI 方面的预防性功效。我们的研究结果表明了富勒烯醇在减轻 AKI 方面的巨大潜力。具体来说,富勒烯醇主要通过抑制肾脏脂质过氧化和亚铁积累来发挥其保护作用,而这正是铁变态反应的两大特征。值得注意的是,富勒烯醇能显著抑制参与顺铂诱导的细胞内脂质过氧化的关键酶的上调,包括酰基-coA 合成酶长链家族成员 4 (ACSL4)、花生四烯酸脂氧合酶 3 (ALOXE3) 和细胞色素 P450 氧化还原酶 (POR),并增强抗氧化系统 xc-/谷胱甘肽 (GSH)/ 谷胱甘肽过氧化物酶 4 (GPX4)。富勒烯醇还能明显抑制铁调节相关基因 mRNA 表达的增加,并防止 AKI 小鼠肾组织中低价铁水平的升高。总之,我们的研究表明富勒烯醇是一种在临床环境中预防 AKI 的有前途的候选药物,并为治疗各种铁中毒相关疾病提供了有价值的见解。
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引用次数: 0
Ultrasmall gold-encapsulated mesoporous platinum to promote photodynamic/catalytic therapy through cascade enzyme-like reactions 超小型金封装介孔铂通过级联酶反应促进光动力/催化治疗
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-03 DOI: 10.1016/j.jcis.2024.11.008
Tianyou Wang , Tao Liu , Zekai Li , Di Wu , Xiaolong Zhao , Leyong Zeng
Mesoporous platinum (mPt) nanozyme possessed enzyme-like property of catalase (CAT) and peroxidase (POD), but the insufficient hydrogen peroxide (H2O2) concentration severely restricted its application in photodynamic therapy (PDT) and catalytic therapy. Herein, by depositing ultrasmall gold nanoparticles (AuNPs) and modifying photosensitizer IR808, a multifunctional nanozyme (mPt@Au-IR808) was designed to promote PDT/catalytic therapy through cascade enzyme-like reactions of glucose oxidase (GOx) and CAT/POD. In tumor microenvironment, the CAT-like oxygen (O2) generation improved the PDT efficacy, and the POD-like hydroxyl radical (·OH) generation achieved endogenous catalytic therapy. Using the GOx/CAT-like activities and endogenous H2O2, the yields of singlet oxygen and ·OH were significantly promoted. Furthermore, mPt@Au-IR808 showed higher photothermal conversion efficiency (41.2%) than mPt (36.1%). By combining the photothermal therapy and enhanced PDT/catalytic therapy, the developed mPt@Au-IR808 nanozyme showed excellent anti-tumor efficacy, which will be promising as cascade nanozyme to promote photo/catalytic therapy.
介孔铂(mPt)纳米酶具有类似过氧化氢酶(CAT)和过氧化物酶(POD)的酶特性,但过氧化氢(H2O2)浓度不足严重限制了其在光动力疗法(PDT)和催化疗法中的应用。本文通过沉积超小金纳米颗粒(AuNPs)和修饰光敏剂IR808,设计了一种多功能纳米酶(mPt@Au-IR808),通过葡萄糖氧化酶(GOx)和CAT/POD的级联酶样反应促进光动力疗法/催化疗法。在肿瘤微环境中,CAT 类氧(O2)生成提高了 PDT 疗效,而 POD 类羟自由基(-OH)生成实现了内源性催化治疗。利用 GOx/CAT 类活性和内源性 H2O2,单线态氧和 -OH 的产量得到了显著提高。此外,mPt@Au-IR808 的光热转换效率(41.2%)高于 mPt(36.1%)。通过将光热疗法与增强光导/催化疗法相结合,所开发的mPt@Au-IR808纳米酶显示出卓越的抗肿瘤功效,有望成为促进光导/催化疗法的级联纳米酶。
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引用次数: 0
Molybdenum-doping to enhance the deprotonation ability of nickel-based hydroxide electrocatalysts for ethanol oxidation 掺钼增强镍基氢氧化物电催化剂在乙醇氧化过程中的去质子化能力。
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-02 DOI: 10.1016/j.jcis.2024.10.197
Ya Tang , Hongzhan Chen , Xueqi Chen , Lijie Zhu , Yanting Ye , Dengke Zhang , Wenyu Huang , Fangyan Xie , Jian Chen , Nan Wang , Yanshuo Jin , Hui Meng
With technological advancements, the practical application of ethanol oxidation reaction (EOR) is becoming increasingly promising, yet the need for higher ethanol concentrations highlights the growing importance of the deprotonation ability (Ni2+ to Ni3+) of the catalyst. The deprotonation ability is the key step for nickel-based catalysts in EOR, as it is essential for Ni2+ to continuously undergo deprotonation to transform into Ni3+ in order to maintain the continuous EOR. Herein, we developed Mo-doped Ni(OH)2 nanosheets by a hydrothermal method. The Mo-doped Ni(OH)2 nanosheets show excellent EOR performance due to the high valence doping of Mo, the onset potential of the oxidation peak (Ni2+ to Ni3+) appears at a position with a small overpotential,. The in-situ Raman spectroscopy technique further characterized the increase in NiOOH in the process of EOR. The Mo-doped Ni(OH)2 nanocomposite catalyst facilitates the oxidation of Ni2+ into Ni3+. Based on the above theoretical guidance, Mo-doped Fe/Ni(OH)2 nanosheets was designed and synthesized. The outstanding EOR performance of the Mo-Fe/Ni(OH)2-3 showed a potential of 1.352 V at 10 mA cm−2. The catalyst was used to design three-electrode reversible zinc-ethanol-air battery (T-RZEAB), which effectively overcomes the opposing kinetic and thermodynamic requirements for EOR and oxygen reduction reaction (ORR) catalysts in the oxygen electrode. The charging voltage of T-RZEAB with Mo-Fe/Ni(OH)2-3 is 240 mV lower than that of a traditional zinc-air battery at 25 mA cm−2.
随着技术的进步,乙醇氧化反应(EOR)的实际应用前景越来越广阔,但由于需要更高浓度的乙醇,催化剂的去质子化能力(Ni2+ 到 Ni3+)变得越来越重要。去质子化能力是镍基催化剂在 EOR 中的关键步骤,因为 Ni2+ 必须不断进行去质子化转化为 Ni3+,才能维持持续的 EOR。在此,我们采用水热法开发了掺杂 Mo 的 Ni(OH)2 纳米片。由于掺杂了高价态的 Mo,氧化峰(Ni2+ 到 Ni3+)的起始电位出现在过电位较小的位置,因此掺杂 Mo 的 Ni(OH)2 纳米片显示出优异的 EOR 性能。原位拉曼光谱技术进一步确定了 EOR 过程中 NiOOH 增加的特征。掺杂 Mo 的 Ni(OH)2 纳米复合催化剂促进了 Ni2+ 氧化成 Ni3+。根据上述理论指导,设计并合成了掺杂 Mo 的 Fe/Ni(OH)2 纳米片。Mo-Fe/Ni(OH)2-3 在 10 mA cm-2 时的电位为 1.352 V,具有出色的 EOR 性能。该催化剂被用于设计三电极可逆锌-乙醇-空气电池(T-RZEAB),有效地克服了氧电极对EOR和氧还原反应(ORR)催化剂的动力学和热力学要求相反的问题。在 25 mA cm-2 的条件下,使用 Mo-Fe/Ni(OH)2-3 的 T-RZEAB 的充电电压比传统锌-空气电池低 240 mV。
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引用次数: 0
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Journal of Colloid and Interface Science
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